Polymeric coatings with oxygen barrier properties are an important technology in food packaging that can extend the shelf life of food products and reduce waste. Although a typical technology in practical use is the deposition of metal or inorganic materials between multilayer films to reduce the oxygen transmission rate, once the film is damaged, oxygen permeates through the damaged area, damaging the packaged food. In addition, nanobrick wall structures consisting of nanoplatelet bricks have the potential to replace barrier films made of inorganic materials, however, they similarly lack repair performance or have slow repair speed despite having repair performance. Inspired by the rapid self-repair mechanism of cephalopods, the study develops a nanoclay-containing coating that can rapidly repair surface damage via water. By introducing CaCl<sub>2</sub>-derived counterions and montmorillonite for nanobrick wall structures into polyelectrolyte multilayers stacked by layer-by-layer self-assembly, the non-covalent polymer network is increased, resulting in mimicking a strong cephalopod-derived β-sheet structure and non-covalent intermolecular interactions derived from cephalopods. Regardless of the amount of montmorillonite added, the self-healing process was completed within 10 sec. The high-water retention at the surface showed super-bubble-phobicity in water and inhibited gas permeation. The oxygen permeability of the coatings with more than a certain amount of montmorillonite was less than 1/100 of that of bare polyethylene. The ultra-fast self-healing gas barrier coating has the potential to be used not only for food products but also for electronics and pharmaceutical packaging and gas separation applications. The key technology developed in this study provides novel insights into the construction of self-healing membranes made of composite materials and will contribute to the formation of a sustainable society.
Fast Self-Healing of Polyelectrolyte Multilayer Nanocoating and Restoration of Super Oxygen Barrier